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Optical nonlinearities, one of the most fascinating properties of two-dimensional (2D) materials, are essential for exploring novel physics in 2D systems and developing next-generation nonlinear optical applications. While tremendous efforts have been made to discover and optimize second-order nonlinear optical responses in various 2D materials, higher odd-order nonlinear processes, which are in general much less efficient than second order ones, have been paid less attention despite their scientific and applicational significance. Here we report giant odd-order nonlinear optical wave mixing in a correlated van der Waals insulator MnPSe3 at room temperature. Illuminated by two near-infrared femtosecond lasers simultaneously, it generates a series of degenerate and non-degenerate four- and six-wave mixing outputs, with conversion efficiencies up to the order of $10^{-4}$ and $10^{-6}$ for the four- and six-wave mixing processes, respectively, far exceeding the efficiencies of several prototypical nonlinear optical materials (GaSe, LiNbO3). This work highlights the intriguing prospect of transition metal phosphorous trichalcogenides for future research of the nonlinear light matter interactions in 2D systems and for potential nonlinear photonic applications., Comment: 17 pages, 4 figures

Optical neural networks (ONNs) herald a new era in information and communication technologies and have implemented various intelligent applications. In an ONN, the activation function (AF) is a crucial component determining the network performances and on-chip AF devices are still in development. Here, we first demonstrate on-chip reconfigurable AF devices with phase activation fulfilled by dual-functional graphene/silicon (Gra/Si) heterojunctions. With optical modulation and detection in one device, time delays are shorter, energy consumption is lower, reconfigurability is higher and the device footprint is smaller than other on-chip AF strategies. The experimental modulation voltage (power) of our Gra/Si heterojunction achieves as low as 1 V (0.5 mW), superior to many pure silicon counterparts. In the photodetection aspect, a high responsivity of over 200 mA/W is realized. Special nonlinear functions generated are fed into a complex-valued ONN to challenge handwritten letters and image recognition tasks, showing improved accuracy and potential of high-efficient, all-component-integration on-chip ONN. Our results offer new insights for on-chip ONN devices and pave the way to high-performance integrated optoelectronic computing circuits.

Optical phase-matching involves establishing a proper phase relationship between the fundamental and generated waves to enable efficient optical parametric processes. It is typically achieved through either birefringence or periodically assigned polarization. Here, we report that twist angle in two-dimensional (2D) materials can generate a nonlinear Berry optical phase to compensate the phase mismatch in the process of nonlinear optical frequency conversion, and the vertical assembly of 2D layers with a proper twist sequence will generate a nontrivial "twist-phase-matching" (twist-PM) regime. The twist-PM model offers superior flexibility in the design of optical crystals, which works for twisted layers with either periodic or random thickness distribution. The designed crystals from twisted rhombohedra boron nitride films give rise to a second-harmonic generation conversion efficiency of ~8% within a thickness of only 3.2 um, and a facile polarization controllability that is absent in conventional crystals (from linear to left-/right-handed circular/elliptical polarizations). Our methodology establishes a platform for the rational designing and atomic manufacturing of nonlinear optical crystals based on abundant 2D materials for various functionalities.

Missing second-order nonlinearity in centrosymmetric graphene overshadows its intriguing optical attribute. Here, we report redox-governed charge doping could effectively break the centrosymmetry of bilayer graphene (BLG), enabling a strong second harmonic generation (SHG) with a strength close to that of the well-known monolayer MoS2. Verified from control experiments with in situ electrical current annealing and electrically gate-controlled SHG, the required centrosymmetry breaking of the emerging SHG arises from the charge-doping on the bottom layer of BLG by the oxygen/water redox couple. Our results not only reveal that charge doping is an effective way to break the inversion symmetry of BLG despite its strong interlayer coupling but also indicate that SHG spectroscopy is a valid technique to probe molecular doping on two-dimensional materials.

Hyperbolic metasurfaces based on van der Waals (vdW) materials support propagation of extremely anisotropic polaritons towards nanoscale light compression and manipulation, and thus has great potential in the applications of planar hyperlens, nanolasing, quantum optics and ultrasensitive infrared spectroscopy. Two-dimensional hexagonal boron nitride (h-BN) as a vdW metasurface can manipulate the propagation of hyperbolic polaritons at the level of single atomic layers, possessing higher degree of field confinement and lower losses than the conventional media. However, active manipulation of hyperbolic polaritonic waves in h-BN midinfrared metasurfaces remains elusive. Herein, we provide an effective strategy for constructing tunable mid-infrared hyperbolic vdW metasurfaces (HMSs). They are composed of meta-atoms that are the in-plane heterostructures of thin-layer h-BN and monolayer graphene strips (iHBNG). The strong coupling of h-BN phonons and graphene plasmons enables the large tunability of light fields by tailoring chemical potentials of graphene without frequency shift, which involves topological transitions of polaritonic modes, unidirectional polariton propagation and local-density-of-state enhancement. Simulated visual near-field distributions of iHBNG metasurfaces reveal the unique transformations of hyperbolic polariton propagations, distinguished from that of individual h-BN and graphene metasurfaces. Our findings provide a platform of optical nanomanipulation towards emerging on-chip polaritonic devices., Comment: 23 pages, 4 figures

Hyperbolic phonon polaritons (HPhPs) in orthorhombic-phase molybdenum trioxide ($\alpha$-MoO3) show in-plane hyperbolicity, great wavelength compression and ultra-long lifetime, therefore holding great potential in nanophotonic applications. However, its polaritonic response in the far-infrared (FIR) range has long remained unexplored due to challenges in experimental characterization. Here, using monochromated electron energy loss spectroscopy (EELS) in a scanning transmission electron microscope (STEM), we probe HPhPs in $\alpha$-MoO3 in both mid-infrared (MIR) and FIR frequencies and correlate their behaviors with microstructures and orientations. We find that low-structural symmetry leads to various phonon modes and multiple Reststrahlen bands (RBs) over a broad spectral range (over 70 meV) and in different directions (55-63 meV and 119-125 meV along b axis, 68-106 meV along c axis, 101-121 meV along a axis). These HPhPs can be selectively excited by controlling the direction of swift electrons. These findings provide new opportunities in nanophotonic and optoelectronic applications such as directed light propagation, hyperlenses and heat transfer.

Photoemission driven by a strong electric field of near-infrared or visible light, referred to as strong-field photoemission, produces attosecond electron pulses that are synchronized to the waveform of the incident light, and this principle lies at the heart of current attosecond technologies. However, full access to strong-field photoemission regimes at near-infrared wavelengths based on solid-state materials is restricted by space-charge screening and material damage at high optical-field strengths, which significantly hampers the realization of predicted attosecond technologies, such as ultra-sensitive optical phase modulation. Here, we demonstrate a new type of strong-field photoemission behaviour with extreme nonlinearity -- photoemission current scales follow a 40th power law of the optical-field strength, making use of sub-nanometric carbon nanotubes and 800 nm pulses. As a result, the total photoemission current depends on the carrier-envelope phase with a greatly improved photoemission current modulation depth of up to 100%, which has not previously been achieved. Time-dependent density functional calculations reveal the completely new behaviour of the optical-field induced tunnelling emission process directly from the valence band of the carbon nanotubes, which is an indication of full access to a strong-field photoemission regime. Furthermore, the nonlinear dynamics are observed to be tunable by changing the binding energy of the valence-band-maximum, as confirmed by Simpleman model calculations. We believe that such extreme nonlinear photoemission from nanotips offers a new means of producing extreme temporal-spatial resolved electron pulses. These results additionally provide a new design philosophy for attosecond electronics and optics by making use of tunable band structures in nanomaterials.

Ultrafast electron pulses, combined with laser-pump and electron-probe technologies, allow for various forms of ultrafast microscopy and spectroscopy to elucidate otherwise challenging to observe physical and chemical transitions. However, the pursuit of simultaneous ultimate spatial and temporal resolution has been largely subdued by the low monochromaticity of the electron pulses and their poor phase synchronization to the optical excitation pulses. State-of-the-art photon-driven sources have good monochromaticity but poor phase synchronization. In contrast, field-driven photoemission has much higher light phase synchronization, due to the intrinsic sub-cycle emission dynamics, but poor monochromaticity. Such sources suffer from larger electron energy spreads (3 - 100 eV) attributed to the relatively low field enhancement of the conventional metal tips which necessitates long pump wavelengths (> 800 nm) in order to gain sufficient ponderomotive potential to access the field-driven regime. In this work, field-driven photoemission from ~1 nm radius carbon nanotubes excited by a femtosecond laser at a short wavelength of 410 nm has been realized. The energy spread of field-driven electrons is effectively compressed to 0.25 eV outperforming all conventional ultrafast electron sources. Our new nanotube-based ultrafast electron source opens exciting prospects for attosecond imaging and emerging light-wave electronics.

In chiral sum frequency generation (C-SFG), the chiral nature of ${\chi}^{(2)}$ requires the three involved electric fields to be pairwise non-parallel, leading to the traditional non-collinear configuration which is a hindrance for achieving diffraction limited resolution while utilizing it as a label-free imaging contrast mechanism . Here we propose a collinear C-SFG (CC-SFG) microscopy modality by using longitudinal z-polarized vectorial field. Label-free chiral imaging with enhanced spatial resolution (~1.4 times improvement in one lateral and the longitudinal directions over the traditional non-collinear scheme) is demonstrated, providing a new path for SFG microscopy with diffraction-limited resolution for mapping chirality., Comment: 7 pages, 4 figures

The optical absorption spectrums of nanomotors made from double-wall carbon nanotubes have been calculated with the time-dependent density functional based tight binding method. When the outer short tube of the nanomotor moves along or rotates around the inner long tube, the peaks in the spectrum will gradually evolve and may shift periodically, the amplitude of which can be as large as hundreds of meV. We show that the features and behaviors of the optical absorption spectrum could be used to monitor the mechanical motions of the double-wall carbon nanotube based nanomotor., Comment: 5 pages; 4 figures

Infrared spectroscopy, especially for molecular vibrations in the fingerprint region between 600 and 1500 cm-1, is a powerful characterization method for bulk materials. However, molecular fingerprinting at the nanoscale level still remains a significant challenge, due to weak light-matter interaction between micron-wavelengthed infrared light and nano-sized molecules. Here, we demonstrate molecular fingerprinting at the nanoscale level using our specially designed graphene plasmonic structure on CaF2 nanofilm. This structure not only avoids the plasmon-phonon hybridization, but also provides in situ electrically-tunable graphene plasmon covering the entire infrared fingerprint region, which was previously unattainable. In addition, undisturbed and highly-confined graphene plasmon offers simultaneous detection of in-plane and out-of-plane vibrational modes with ultrahigh detection sensitivity down to the sub-monolayer level, significantly pushing the current detection limit of far-field mid-infrared spectroscopy. Our results provide a platform, fulfilling the long-awaited expectation of high sensitivity and selectivity far-field fingerprint detection of nano-scale molecules for numerous applications., Comment: 20 pages, 6 figures, accepted by Nature Communications